The Role of Dual-Interfaces on Structural Reconstruction of Cobalt–Zinc–Indium Catalysts for CO2 Hydrogenation

Surface reconstruction of heterogeneous catalysts plays a critical role in determining their catalytic performance, yet controlling dynamic structural evolution remains challenging. Reconstructions are typically focused on alterations of the metal–support interactions. Herein, we reveal a dual–interface synergistic modulation strategy by introducing Co-ZnO_x interfaces to stabilize Co-In₂O_3–x active sites in cobalt–indium catalysts for CO₂ hydrogenation. Through in situ XRD, quasi-in situ XPS, and DFT simulations, it was demonstrated that this way protected the Co-In₂O_3–x interfaces from structural transformations to Co₃InC_0.75 and CoIn₂, and oxygen vacancies in the support regulated the uniform distribution of dual-interface, synergistically enhancing CO₂ activation and stabilizing the key intermediate HCOO*. At 280 °C, the optimized CoZnIn-P catalyst achieves a methanol space-time yield of 0.92 g_methanol g_catalyst^–1 h^–1, outperforming previously reported catalysts. This work provides a paradigm for designing multicomponent catalysts with controlled reconstruction dynamics, emphasizing the pivotal role of interface engineering in methanol synthesis.